All primary data files of the journal article mentioned can be found here. The data is structured by the materials, electrodes, and models. The characterization data of each precursor and COF are located in the subfolders "Co(tapp)", "Co(ttpp)", "COF-A", "COF-T", "COF-367-Co", and "Co(tapp)-TPDA-COF". The characterization and catalysis data of electrodes are located in the subfolder "Electrodes". The structural model data are located in the subfolder "Modeling". The characterization and catalysis data are recorded experimentally. The structure model data are created by manual modeling and Rietveld refinement. The characterization and catalysis data can be used to replicate the experiments and to evaluate and compare the materials' properties with others. The structure model data can be used to investigate the materials' structures and to predict properties by computation.